Pd-based catalysts are widely used in the oxidation of CH4 and have a significant impact on global warming. However, understanding their active sites remains controversial, because interconversion between Pd and PdO occurs consecutively during the reaction. Understanding the intrinsic active sites under reaction conditions is critical for developing highly active and selective catalysts. In this study, we demonstrated that partially oxidized palladium (PdOx) on the surface plays an important role for CH4 oxidation. Regardless of whether the initial state of Pd corresponds to oxides or metallic clusters, the topmost surface is PdOx, which is formed during CH4 oxidation. A quantitative analysis using CO titration, diffuse reflectance infrared Fourier-transform spectroscopy, X-ray diffraction, and scanning transmission electron microscopy demonstrated that a surface PdO layer was formed on top of the metallic Pd clusters during the CH4 oxidation reaction. Furthermore, the time-on-stream test of CH4 oxidation revealed that the presence of the PdO layer on top of the metallic Pd clusters improves the catalytic activity. Our periodic density functional theory (DFT) calculations with a PdOx slab and nanoparticle models aided the elucidation of the structure of the experimental PdO particles, as well as the experimental C-O bands. The DFT results also revealed the formation of a PdO layer on the metallic Pd clusters. This study helps achieve a fundamental understanding of the active sites of Pd and PdO for CH4 oxidation and provides insights into the development of active and durable Pd-based catalysts through molecular-level design.
机构:
Univ Calif Berkeley, Lawrence Berkeley Lab, Div Chem Sci, Berkeley, CA 94720 USAUniv Calif Berkeley, Lawrence Berkeley Lab, Div Chem Sci, Berkeley, CA 94720 USA
Su, SC
Carstens, JN
论文数: 0引用数: 0
h-index: 0
机构:Univ Calif Berkeley, Lawrence Berkeley Lab, Div Chem Sci, Berkeley, CA 94720 USA
Carstens, JN
Bell, AT
论文数: 0引用数: 0
h-index: 0
机构:Univ Calif Berkeley, Lawrence Berkeley Lab, Div Chem Sci, Berkeley, CA 94720 USA
机构:
Univ Buffalo State Univ New York, Dept Chem & Biol Engn, Buffalo, NY 14260 USAUniv Buffalo State Univ New York, Dept Chem & Biol Engn, Buffalo, NY 14260 USA
Chen, Junjie
Giewont, Kevin
论文数: 0引用数: 0
h-index: 0
机构:
Univ Buffalo State Univ New York, Dept Chem & Biol Engn, Buffalo, NY 14260 USAUniv Buffalo State Univ New York, Dept Chem & Biol Engn, Buffalo, NY 14260 USA
Giewont, Kevin
Walker, Eric A.
论文数: 0引用数: 0
h-index: 0
机构:
Univ Buffalo State Univ New York, Inst Computat & Data Sci, Buffalo, NY 14260 USAUniv Buffalo State Univ New York, Dept Chem & Biol Engn, Buffalo, NY 14260 USA
Walker, Eric A.
Lee, Jungkuk
论文数: 0引用数: 0
h-index: 0
机构:
Univ Buffalo State Univ New York, Dept Chem & Biol Engn, Buffalo, NY 14260 USAUniv Buffalo State Univ New York, Dept Chem & Biol Engn, Buffalo, NY 14260 USA
Lee, Jungkuk
Niu, Yubiao
论文数: 0引用数: 0
h-index: 0
机构:
Swansea Univ, Coll Engn, Swansea SA1 8EN, W Glam, WalesUniv Buffalo State Univ New York, Dept Chem & Biol Engn, Buffalo, NY 14260 USA
Niu, Yubiao
Kyriakidou, Eleni A.
论文数: 0引用数: 0
h-index: 0
机构:
Univ Buffalo State Univ New York, Dept Chem & Biol Engn, Buffalo, NY 14260 USAUniv Buffalo State Univ New York, Dept Chem & Biol Engn, Buffalo, NY 14260 USA
机构:
Nagoya Univ, Grad Sch Engn, Nagoya, Aichi 4648603, JapanNagoya Univ, Grad Sch Engn, Nagoya, Aichi 4648603, Japan
Mahara, Yuji
Murata, Kazumasa
论文数: 0引用数: 0
h-index: 0
机构:
Nagoya Univ, Grad Sch Engn, Nagoya, Aichi 4648603, JapanNagoya Univ, Grad Sch Engn, Nagoya, Aichi 4648603, Japan
Murata, Kazumasa
Ueda, Kakuya
论文数: 0引用数: 0
h-index: 0
机构:
Nagoya Univ, Grad Sch Engn, Nagoya, Aichi 4648603, JapanNagoya Univ, Grad Sch Engn, Nagoya, Aichi 4648603, Japan
Ueda, Kakuya
Ohyama, Junya
论文数: 0引用数: 0
h-index: 0
机构:
Nagoya Univ, Grad Sch Engn, Nagoya, Aichi 4648603, Japan
Kyoto Univ, Unit Elements Strategy Initiat Catalysts Batterie, Kyoto 6158530, JapanNagoya Univ, Grad Sch Engn, Nagoya, Aichi 4648603, Japan
Ohyama, Junya
Kato, Kazuo
论文数: 0引用数: 0
h-index: 0
机构:
Japan Synchrotron Radiat Res Inst, 1-1 Kouto, Sayo, Hyogo 6795198, JapanNagoya Univ, Grad Sch Engn, Nagoya, Aichi 4648603, Japan
Kato, Kazuo
Satsuma, Atsushi
论文数: 0引用数: 0
h-index: 0
机构:
Nagoya Univ, Grad Sch Engn, Nagoya, Aichi 4648603, Japan
Kyoto Univ, Unit Elements Strategy Initiat Catalysts Batterie, Kyoto 6158530, JapanNagoya Univ, Grad Sch Engn, Nagoya, Aichi 4648603, Japan
机构:
Zhejiang Univ, Sch Mat Sci & Engn, Ctr Electron Microscopy, Hangzhou 310027, Peoples R China
Zhejiang Univ, Sch Mat Sci & Engn, State Key Lab Silicon Mat, Hangzhou 310027, Peoples R ChinaZhejiang Univ, Sch Mat Sci & Engn, Ctr Electron Microscopy, Hangzhou 310027, Peoples R China
Chen, Shiyuan
Li, Songda
论文数: 0引用数: 0
h-index: 0
机构:
Zhejiang Univ, Sch Mat Sci & Engn, Ctr Electron Microscopy, Hangzhou 310027, Peoples R China
Zhejiang Univ, Sch Mat Sci & Engn, State Key Lab Silicon Mat, Hangzhou 310027, Peoples R ChinaZhejiang Univ, Sch Mat Sci & Engn, Ctr Electron Microscopy, Hangzhou 310027, Peoples R China
Li, Songda
You, Ruiyang
论文数: 0引用数: 0
h-index: 0
机构:
Zhejiang Univ, Sch Mat Sci & Engn, Ctr Electron Microscopy, Hangzhou 310027, Peoples R China
Zhejiang Univ, Sch Mat Sci & Engn, State Key Lab Silicon Mat, Hangzhou 310027, Peoples R ChinaZhejiang Univ, Sch Mat Sci & Engn, Ctr Electron Microscopy, Hangzhou 310027, Peoples R China
You, Ruiyang
Guo, Ziyi
论文数: 0引用数: 0
h-index: 0
机构:
Univ New South Wales, Sch Chem Engn, Sydney, NSW 2052, AustraliaZhejiang Univ, Sch Mat Sci & Engn, Ctr Electron Microscopy, Hangzhou 310027, Peoples R China
Guo, Ziyi
Wang, Fei
论文数: 0引用数: 0
h-index: 0
机构:
Zhejiang Univ, Sch Mat Sci & Engn, Ctr Electron Microscopy, Hangzhou 310027, Peoples R China
Zhejiang Univ, Sch Mat Sci & Engn, State Key Lab Silicon Mat, Hangzhou 310027, Peoples R ChinaZhejiang Univ, Sch Mat Sci & Engn, Ctr Electron Microscopy, Hangzhou 310027, Peoples R China
Wang, Fei
Li, Guanxing
论文数: 0引用数: 0
h-index: 0
机构:
Zhejiang Univ, Sch Mat Sci & Engn, Ctr Electron Microscopy, Hangzhou 310027, Peoples R China
Zhejiang Univ, Sch Mat Sci & Engn, State Key Lab Silicon Mat, Hangzhou 310027, Peoples R ChinaZhejiang Univ, Sch Mat Sci & Engn, Ctr Electron Microscopy, Hangzhou 310027, Peoples R China
Li, Guanxing
Yuan, Wentao
论文数: 0引用数: 0
h-index: 0
机构:
Zhejiang Univ, Sch Mat Sci & Engn, Ctr Electron Microscopy, Hangzhou 310027, Peoples R China
Zhejiang Univ, Sch Mat Sci & Engn, State Key Lab Silicon Mat, Hangzhou 310027, Peoples R ChinaZhejiang Univ, Sch Mat Sci & Engn, Ctr Electron Microscopy, Hangzhou 310027, Peoples R China
Yuan, Wentao
Zhu, Beien
论文数: 0引用数: 0
h-index: 0
机构:
Chinese Acad Sci, Shanghai Adv Res Inst, Zhangjiang Lab, Shanghai 201210, Peoples R China
Chinese Acad Sci, Shanghai Inst Appl Phys, Key Lab Interfacial Phys & Technol, Shanghai 201800, Peoples R ChinaZhejiang Univ, Sch Mat Sci & Engn, Ctr Electron Microscopy, Hangzhou 310027, Peoples R China
Zhu, Beien
Gao, Yi
论文数: 0引用数: 0
h-index: 0
机构:
Chinese Acad Sci, Shanghai Adv Res Inst, Zhangjiang Lab, Shanghai 201210, Peoples R China
Chinese Acad Sci, Shanghai Inst Appl Phys, Key Lab Interfacial Phys & Technol, Shanghai 201800, Peoples R ChinaZhejiang Univ, Sch Mat Sci & Engn, Ctr Electron Microscopy, Hangzhou 310027, Peoples R China
Gao, Yi
Zhang, Ze
论文数: 0引用数: 0
h-index: 0
机构:
Zhejiang Univ, Sch Mat Sci & Engn, Ctr Electron Microscopy, Hangzhou 310027, Peoples R China
Zhejiang Univ, Sch Mat Sci & Engn, State Key Lab Silicon Mat, Hangzhou 310027, Peoples R ChinaZhejiang Univ, Sch Mat Sci & Engn, Ctr Electron Microscopy, Hangzhou 310027, Peoples R China
Zhang, Ze
Yang, Hangsheng
论文数: 0引用数: 0
h-index: 0
机构:
Zhejiang Univ, Sch Mat Sci & Engn, Ctr Electron Microscopy, Hangzhou 310027, Peoples R China
Zhejiang Univ, Sch Mat Sci & Engn, State Key Lab Silicon Mat, Hangzhou 310027, Peoples R ChinaZhejiang Univ, Sch Mat Sci & Engn, Ctr Electron Microscopy, Hangzhou 310027, Peoples R China
Yang, Hangsheng
Wang, Yong
论文数: 0引用数: 0
h-index: 0
机构:
Zhejiang Univ, Sch Mat Sci & Engn, Ctr Electron Microscopy, Hangzhou 310027, Peoples R China
Zhejiang Univ, Sch Mat Sci & Engn, State Key Lab Silicon Mat, Hangzhou 310027, Peoples R ChinaZhejiang Univ, Sch Mat Sci & Engn, Ctr Electron Microscopy, Hangzhou 310027, Peoples R China
机构:
Gwangju Inst Sci & Technol, Res Ctr Innovat Energy & Carbon Optimized Synth C, 123 Cheomdan Gwagiro, Gwangju 61005, South Korea
Gwangju Inst Sci & Technol, Sch Earth Sci & Environm Engn, Gwangju Inst Sci & Technol, 123 Cheomdan Gwagiro, Gwangju 61005, South KoreaGwangju Inst Sci & Technol, Res Ctr Innovat Energy & Carbon Optimized Synth C, 123 Cheomdan Gwagiro, Gwangju 61005, South Korea
Park, Jiseok
Kim, Dongjoon
论文数: 0引用数: 0
h-index: 0
机构:
Ohio State Univ, William G Lowrie Chem & Biomol Engn, Columbus, OH 43210 USAGwangju Inst Sci & Technol, Res Ctr Innovat Energy & Carbon Optimized Synth C, 123 Cheomdan Gwagiro, Gwangju 61005, South Korea
Kim, Dongjoon
Byun, Sang Woo
论文数: 0引用数: 0
h-index: 0
机构:
Gwangju Inst Sci & Technol, Res Ctr Innovat Energy & Carbon Optimized Synth C, 123 Cheomdan Gwagiro, Gwangju 61005, South Korea
Gwangju Inst Sci & Technol, Sch Earth Sci & Environm Engn, Gwangju Inst Sci & Technol, 123 Cheomdan Gwagiro, Gwangju 61005, South KoreaGwangju Inst Sci & Technol, Res Ctr Innovat Energy & Carbon Optimized Synth C, 123 Cheomdan Gwagiro, Gwangju 61005, South Korea
Byun, Sang Woo
Shin, Hyeonwoo
论文数: 0引用数: 0
h-index: 0
机构:
Gwangju Inst Sci & Technol, Res Ctr Innovat Energy & Carbon Optimized Synth C, 123 Cheomdan Gwagiro, Gwangju 61005, South Korea
Gwangju Inst Sci & Technol, Sch Earth Sci & Environm Engn, Gwangju Inst Sci & Technol, 123 Cheomdan Gwagiro, Gwangju 61005, South KoreaGwangju Inst Sci & Technol, Res Ctr Innovat Energy & Carbon Optimized Synth C, 123 Cheomdan Gwagiro, Gwangju 61005, South Korea
Shin, Hyeonwoo
Ju, Yanggeun
论文数: 0引用数: 0
h-index: 0
机构:
Gwangju Inst Sci & Technol, Res Ctr Innovat Energy & Carbon Optimized Synth C, 123 Cheomdan Gwagiro, Gwangju 61005, South Korea
Gwangju Inst Sci & Technol, Sch Earth Sci & Environm Engn, Gwangju Inst Sci & Technol, 123 Cheomdan Gwagiro, Gwangju 61005, South KoreaGwangju Inst Sci & Technol, Res Ctr Innovat Energy & Carbon Optimized Synth C, 123 Cheomdan Gwagiro, Gwangju 61005, South Korea
Ju, Yanggeun
Min, Haehyun
论文数: 0引用数: 0
h-index: 0
机构:
Gwangju Inst Sci & Technol, Res Ctr Innovat Energy & Carbon Optimized Synth C, 123 Cheomdan Gwagiro, Gwangju 61005, South Korea
Gwangju Inst Sci & Technol, Sch Earth Sci & Environm Engn, Gwangju Inst Sci & Technol, 123 Cheomdan Gwagiro, Gwangju 61005, South KoreaGwangju Inst Sci & Technol, Res Ctr Innovat Energy & Carbon Optimized Synth C, 123 Cheomdan Gwagiro, Gwangju 61005, South Korea
Min, Haehyun
Kim, Young Jin
论文数: 0引用数: 0
h-index: 0
机构:
Korea Res Inst Chem Technol, Environm & Sustainable Resources Res Ctr, Daejeon 34114, South KoreaGwangju Inst Sci & Technol, Res Ctr Innovat Energy & Carbon Optimized Synth C, 123 Cheomdan Gwagiro, Gwangju 61005, South Korea
Kim, Young Jin
Heo, Iljeong
论文数: 0引用数: 0
h-index: 0
机构:
Korea Res Inst Chem Technol, Environm & Sustainable Resources Res Ctr, Daejeon 34114, South KoreaGwangju Inst Sci & Technol, Res Ctr Innovat Energy & Carbon Optimized Synth C, 123 Cheomdan Gwagiro, Gwangju 61005, South Korea
Heo, Iljeong
Hazlett, Melanie J.
论文数: 0引用数: 0
h-index: 0
机构:
Concordia Univ, Gina Cody Sch Engn & Comp Sci Chem & Mat Engn, Montreal, PQ H4B1R6, CanadaGwangju Inst Sci & Technol, Res Ctr Innovat Energy & Carbon Optimized Synth C, 123 Cheomdan Gwagiro, Gwangju 61005, South Korea
Hazlett, Melanie J.
Kim, Minkyu
论文数: 0引用数: 0
h-index: 0
机构:
Yeungnam Univ, Sch Chem Engn, 280 Daehak ro, Gyongsan 38541, South KoreaGwangju Inst Sci & Technol, Res Ctr Innovat Energy & Carbon Optimized Synth C, 123 Cheomdan Gwagiro, Gwangju 61005, South Korea
Kim, Minkyu
论文数: 引用数:
h-index:
机构:
Kang, Sung Bong
APPLIED CATALYSIS B-ENVIRONMENT AND ENERGY,
2022,
316